Our goal is to provide a comprehensive understanding of structure, dynamics, and reactivity for Lewis acid promoted transformations. Our approach is based on the integration of NMR experiments, computational studies, and synthetic transformations. The multinuclear variable temperature NMR studies will be used to monitor reactions and to characterize the intermediates, dynamics. Computational studies, including molecular modeling, molecular mechanics, semi-empirical and ab initio methods, will assist us in carefully analyzing the geometries, bonding, and energies associated with the three-dimensional complexes. The completion of these studies will include performing synthetic transformations to support our spectroscopic and computational findings. The organic substrates chosen for these studies are readily available and structurally simple, yet can yield a variety of structurally diverse Lewis acid complexes. The Lewis acids chosen for these studies offer a range of ligand substitution and are accessible by NMR (with the exception of Ti), which is vital for complete characterization of the possible intermediates. We intend to derive models for synthetically useful transformations based on our NMR studies. The impact of our studies will go well beyond the specific systems studied by assisting synthetic chemists in designing and exploring new Lewis acid methodologies for the chemo-, regio-, and stereoselective synthesis of complex molecules.